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or mechanical. If successful, these functions can be responsive to or modulated by local cues in the device, e.g., spikes in electric fields, harsh thermal gradients, or extreme heterogeneities in ionic or electronic current. In this way, the implementation of responsive and reconfigurable interphases may make available new behaviors within the device that are adaptive or even self-rectifying with the intent of minimizing energetic losses or chemical degradation over time. A coordinated future direction focused on molecularly tailored interfaces with active or adaptive transport behaviors represents an important departure from the majority of today’s state-of-the-art strategies, which are decidedly passive.61 Discovery of new chemistries with switchable functionality (e.g., metal-insulator, semiconductor-insulator, ion conductor-ionic insulator, thermal conductor-thermal insulator, redox-mediating, shape-changing, etc.) that gate the transport behavior of energy carriers (e.g., electrons, ions, phonons, mass, etc.) could be transformative with respect to carrier transport under specific conditions or upon application of an external stimulus, both locally and globally.62 Success hinges upon the ability to initiate or arrest the formation and growth of the interphase responsible for charge transfer under conditions relevant to use of the battery. To guide the design of such concepts, new predictive tools are needed to direct the choice of materials, with validation provided by interface-specific operando analytical techniques. Presently lacking is a reliable theoretical framework for modeling charge transfer at an atomically defined heteromaterial interface (e.g., liquid-solid, liquid-semi-solid, and solid-solid) at the nanoscale. Research of the future will need to appreciate, in turn, the value of incorporating bias in a theoretical framework, which will certainly alter the free-energy landscape for charge transfer and transport. The impact of a coordinated effort in understanding and controlling interphases (and their interfaces) will reveal new paths to significantly enhance cycle life, rate capability, and energy density, as these are among the properties in the cell that most critically depend on charge transfer across and charge transport along such interfaces. Furthermore, it has not been possible previously to direct the evolution of the interphase or interface in a component of the cell to something that sustains its useful functions indefinitely. Coordinated efforts between experimental, characterization, and modeling efforts stand to reveal the first links between molecular-level processes and bulk electrochemical phenomena. 2.3.2 RESEARCH THRUSTS To address these fundamental challenges at electrochemical interfaces and interphases, two connected research themes emerging over the next decade are envisioned. Integrated experimental and theoretical strategies able to elucidate the complex processes that control electrochemistry and transport at interfaces in their full electrochemical context are a high priority. The second emerging theme seeks to harness knowledge of interphases from best-in-class EES systems, idealized EES systems that serve as model systems, and fully operational EES devices to design electrochemical interfaces and interphases with explicit properties required for performing a desired electrochemical function. Specific opportunities in each of these two themes are highlighted next. Thrust 3a: Unravel Interfacial Complexity through In Situ and Operando Characterization and Theory Unravelling the complexity of coupled processes that control the function of heterogeneous electrochemical interfaces demands new approaches that use combinations of tools for complementary insights. This goal is being pursued through theoretical approaches, the results of which are then verified by in situ probing of the solid-liquid interface through advanced microscopy and spectroscopy. The experimental methods cited below have shown great promise in recent years, and their research trajectory promises continuing development and applications that will propel the frontiers of energy storage science and possibly stimulate innovations not yet conceived. Using these approaches, major advances are envisioned that will provide a mechanistic understanding of the interfacial processes linking morphology and function in EES systems as well as the foundations for directed design of functional electrochemical interfaces. Characterizing Interfacial Phenomena in Functional EES Contexts: At one end of the spectrum, there are opportunities for studies that take advantage of well-controlled model systems in which the functional aspects of the electrochemical cell are preserved. Such studies would enable detailed understanding of how interfaces of well-defined chemistry contribute to overall function. At another extreme, there are opportunities for approaches that enable intrusive ex-situ, in-situ, and operando interrogation of specific features of a heterogeneous interface NEXT GENERATION ELECTRICAL ENERGY STORAGE PRIORITY RESEARCH DIRECTION – 3 47PDF Image | Next Generation Electrical Energy Storage
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